Monte-Carlo simulations are used to calculate the primary radical and molecular yields (
g-values) of water radiolysis versus temperature in the range 25–300°C, for different high linear energy transfer radiations (protons,
2H+, and
7Li3+) up to
65keV/μm. The results are compared, at
10−7 s, to experimental data at 25°C, 95°C, and 180°C. Excellent agreement is obtained for
g(e−aq) and
g(OH) over the whole temperature range, but
g(H2),
[g(H)+g(H2)], and
g(H2O2) are substantially larger than the measured values at 180°C. Our
g-values are also compared with fast-neutron radiolysis yields and with deterministic modeling calculations. The agreement is generally satisfactory.